Process of conducting gaseous catalytic reactions and apparatus therefor



Oct. 2, 1928. 1,686,349

R. E. SLADE PROCESS OF CONDUCTING GASEOUS CATALYTIC REACTIONS AND APPARATUS THEREFOR Filed May 1', 1926 I EL zcne 1c HEATING sus/mvr firmsnn or UwcaMvzR-rni 645 1:

CONVERTER n jfkEfiM af' cmv I/ERI'ED 6/15 v 7 Y INVENTOR 4 TTORNEYS Patented a. 2, 19 8.

UNITED STATES PATENT OFFICE.

ROLAND EDGAR SLLDE, OF BILLINGHAM-ON-TEES, ENGLAND, ASSIGNOB'TO ATMOS- PHEBIC NITROGEN COBPOBATION OF NEW YORK, N. Y., A CORPORATION OF NEW YORK.

PROCESS OI CONDUCTING GASEOUS CATALYTIC REACTIONS AND AIPARATUS THERE- 1'03.

Application fled. Kay 1, 1928, Serial No. 106,166, and in Great Britain Kay 4, 1985.

This invention relates toan improved process andapparatus for the carrying out of gaseous catalytic reactions, particularly reactions, such as the synthesis of ammoma from 5 its elements, which take place at an elevated temperature and with evolution of large quantities of heat.

In carrying out such reactions at elevated temperatures, it is standard practice to conserve the heat of the system by arrangmg that a large part of the available heat of the hot products shall be imparted to the fresh cold reactants, so that the latter may enter the catalytic chamber'at a temperature equal to or not much below that desired in the contact mass. For this purpose a heat interchanger constituting an addition to the catalytic c amber proper) and a heat interchange operation separate from the catalyst mass have as been hitherto employed, but I have now found possible to dispense with such additional heatinterchanger by arranging that a part of the contact mass itself shall act as a regenerator or source of heat for all or a substantial part of the required pre-heatmg of the fresh gas.

The invention is illustrated in the accom-- panying drawingsin which Fig. 1 illustrates one form of my improved catalytic apparatus,

a while Fig. 2 shows diagrammatically a gas reversing mechanism for effecting a reversal of gas flow throu h the catalytic material in the ap aratus of ig. 1.

As own in Fig. 1 the apparatus consists of a cylindrical envelope A closed at the ends by suitable covers B and C to form a pressureresisting chamber. Gas ports D and E are rovided in thecovers B and C respectively. lhe catalytic material K is contained in what 9 may be termed an enclosing chamber by which is meant that chamber or space which determines the shape of the catalyst bed and which may be identical with the inner configuration of the pressure-sustaining envelop A althou h preferably the enclosing chamber is estab ished by lining the inner .walls of the vessel A with heat insulating material F. This lining is preferably of greater thickness towards the middle of the a paratus and tapers toward the ends of t e shell, as indicated in the drawing, and in this way the e H is made of varying cross-section,

Eeing greatest at the ends and smallest in the .middle. The space H is divided intoa numelectrodes M penetrating the walls of the shell through a gastight joint.

In the synthesis of ammonia the working of the apparatus is as follows:

The central catalyst compartment (or whichever compartment is selected for initial heating) is heated to a suitably high temperature, say 500 0., by, for example, an elec trical heating coil such as L. The escape of heat by conduction through the contact mass is prevented by the perforated heat insulating partitions on either side. A nitrogen-hydrogen mixture, usually under substantial pressure, is then introduced into and passed through the a paratus in the direction D'to E, the heater ein kept on until the process is well started. his mixture need not be preheated before entering the apparatus, and may be at ordinary temperature. On meeting the hot art of the contact mass'some nitrogen and ydrogen combineto form ammonia and heat is liberated. On the other hand, the cold gases streaming from D chill the nearer border of thehot zone, and also tend to carry the heat evolved by the reaction in the direction towards E, so that the final result is that the hot reaction zone is displaced more and more towards E and the synthesis is accomplished in this traveling zone. The gases, which of course travel faster than the zone, then traverse the'remaining part of the contact mass, and during this time they are subject to a continually decreasing temperature. Moreover, on account of the shape of the enclosure, the gases travel more slowly towards the outlet and they are therefore a longer time in contact with the catal st than would be the case if the catalyst cham were justcylindrical. This relatively prolonged contact with catalyst at a lower temperature than that of the main synthesis'zone tends to enrich the ammonia content. of the gas, i. e., full advantage. is taken of the synthesizing power of the remainin catalyst. In addition, the end ortion of the d of catalyst takes up nearly a or the desired amount o,the Benresultant gases.

sible heat of the gases and the gaseous resultants therefore pass off at a relatively low temperature, e. g., 100 C.

When the hot zone approaches the end of the apparatus, so that, if the operation is con tinued, the gases will begin to leave while still at a relatively hightemperature, the direction of the gas flow is reversed, and the hot zone now travels back toward the other end of the chamber. This reversal may be effected by means such as are indicated in Fig. 2 where, when valves X, X are closed and valves Y, Y open, the gases flow in the direction of the full line arrows while, when the valves Y, Y are closed and the valves X, X are open, the gas flows in the reverse direction.

By suitably reversing the gas flow the hot zone may be made to travel to and fro between selectable limits, while the remainder, i. e., the temporarily inactive end portions of the contact mass, act as heat regenerators, one end portion preheating the fresh gases to the reaction temperature, and the other end portion absorbing and storing heat from the hot Once started the process is autothermic and needs no external supply of heat, so that after the initial heating period the flow of current through the heating coil L is discontinued. It may even be advisable to removesome of the heat generated within the chamber, and in general this will be the case when the percentage of ammonia synthesized is relatively high. In such a case the excess of heat, which would prevent the maintenance of the optimum temperature, may be removed by cooling means such as water cooled tubes placed within the apparatus. Suitable arrangements are of course made for recording the temperature in the different parts of the apparatus.

If the contact mass were of such a nature that it conducted heat only very slowly, the heat insulating partitions J might be dis pensed with, but with catalysts of a metallic nature the use of insulating partitions or their equivalent is obviously preferred. Of course, the process need not be so conducted as to take place wholly within a single shell or chamber, but may be conducted in a plurality of chambers connected in series. In that case each chamber will correspond to one or more of the catalyst compartments of Fig. 1.

My invention greatly simplifies the apparatus forsynthetic processes such as the synthesis of ammonia from its elements, and simplifies the process'itself. The number of vessels is reduced and their design is simplified.

The ordinary type of heat interchanger with its two series of separate gas passages is relatively complicated and expensive, particularly when high ressures and temperatures and infiamma le gases are involved as in ammonia synthesis. Heat utilization is favored.

In addition, the catalyticreaction itself is improved. By making the heat interchan e or preheatin step continuous with the su sequent catalysis step and by carrying out the preheating step by contacting the gases with hot catalyst material, the conditions for the desired catayltic reaction are at once and always present. So soon as the fresh gases have reached-a reaction temperature, no matter how small the reaction tendency may be, and no matter what the required reaction temperature may be, the reaction begins. With an installation containing separate heat-interchanger and converter units, the temperature in the portions of the exchanger next to the converter may be sufiicient to cause some reaction, but this tendency cannot be utilized as no catalyst is available, i. e. by means of my invention the catalytic reaction proceeds throughout the entire reaction temperature range which prevails durin the entire operation including the so-cal ed preheating, catalysis, and cooling steps or stages.

It will be noted that, although the material between the partitions J is preferably material of the same character throughout, to wit, catalyst material, the arrangement may be modified so that such part of the material as serves primarily as the heat-interchange medium may be constituted of refractory brick or other material which, while possessing the heat-absorbing and transmitting qualities of the catalyst material, is not in or of itself a catalyst. In a similar way various other modifications and variations in detail may obviously be made without departing from the spirit of the invention.

I claim:

1. The process of conducting exothermic gaseous catalytic reactions which comprises preheating a stream of uncatalyzed gases by passing them in contact with a hot body of heat-storing material, conducting said preheated stream of gases in contact with and through a body of catalyst material to cause the exothermic reaction to progress in the direction of the flow of the gases from the region of the inlet end of the said catalyst material toward the region of the exit end thereof, leading the hot catalyzed gases of the. foregoing steps in contact with a second body of heat-storing material to remove heat from said gases, continuing the aforesaid steps until the portion of the catalyst ma.- terial in the region of the exit end is at a higher thermal state than the correspondingly located material of the inlet end and thereupon causing the stream of gases to. flow, in a reversed direction and under the aforesaid operating conditions, first in contact with the heat-storing material of the third step, now in a hot condition, then in contact with the catalyst, as heretofore set forth, and finally in contact with the heat-storing material of the first step in order to re-heat it, and

repeating the aforesaid steps as acontinuous- 1y functioning catalytic procedure with substantially regular reversals of flow of gases.

ever the temperature of the gas exit end of the catalyst bed begins to exceed that which prevailed at the as inlet end of the bed at the time when sai end commenced to serve as the inlet for the gas.

3. The process of conducting exothermic gaseous catalytic reactions which comprises setting up a zone of reaction temperature within the catalyst bed, introducing the gas at one end of the catalyst bed at a temperature substantially below that of the reaction zone, whereb the reaction zone is caused to travel in the irection of flow of the gases and successively reversing the flow whenever l the temperature of the gas exit end of the catalyst bed begins to exceed that which prevailed at the gas inlet end of the bed at the time when said end commenced to serve as the inlet for the gas.

4. A process such as set forth in claim 1 in which both of the bodies of heat-storing material are constituted of material of the same constitution as the intervening catalyst material. 5. A process such as set forth in claim 1 in which the as stream flows with a lower velocity whi e passing through the heat-storing material than while passing through the intervening catalyzing material.

6. The process of conducting exothermic gaseous catalytic reactions which comprises causing a zone of high temperature to oscillate from point adjacent one end of the catalyst body to a point adjacent the other end of said body by maintaining the extreme ends of the bed constantly below that of the reaction zone by introducing the gaseous reactants at temperatures materially below that of the reaction and by alternatin the flow gfdgaseous reactants through sai catalyst 7. The process of carrying out exothermic gaseous catalytic reactions without an ordinary heat interchanger or with cooling in which the fresh cold gases are passed through a bodv of catalyst containing available heat,

and then through a hot zone of the catalyst and finally through a further body of catalyst to which'alarge part of'the available heat is given up, then when the first parts of the cat: alyst have become cold and the last parts sulficiently hot, reversing the direction of gas flow, so that the conditions for the catalytic reaction are once more favorable.

8. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber constricted at its middle portions, catalyst material in the constricted middle portions of said chamber, externally controlled means for heating the catalyst at a constricted portion of the same chamber, heat-storing material at each end of said catalyst body, arranged as heat regenerators, and a gas port operatively associated with each heat regenerator.

9. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber constricted at its IIllCldle portion, catalyst material in the constricted middle portion of said chamber, heatstoring material at each end of said catalyst body arranged as heat regenerators, and a gas port operatively associated with each heat regenerator.

10. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber constricted at its middle portion, catalyst material in the constricted middle portions of said chamber, heat-storin material at each end of said catalyst body arranged as heat regenerators, and a gas port operatively associated with each heat regenerator, the heat-storing material and the intervening catalyst material being constituted throughout of catalyst substance.

11. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber, catalyst material in the middleof said chamber, heat-storing material at each end of said catalyst body arranged as heat regenerators, and a gas port operatively associated with each heat regenerator, the heat-storing material and the intervening catalyst material being constituted throughout of catalyst substance arranged in compartments separated by gaspermeable heat insulating partitions.

12. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber, heat insulating material associated with the inner walls of said chamber and diminishin in thickness tfrom the center to the ends 0? the chamber, and defining the gas passage through said chamber, catalyst material in the middle constricted part of said passage, heat-storing material at the outer wider parts of said passage, and a gas port operatively associated with each of the outer ends of said passage.

13. Apparatus for conducting exothermic gaseous catalytic reactions which comprises an enclosing chamber constricted at its middle portion, catalyst material in the constricted middle portions of said chamber, heat-storin material at each end of said catalyst body arranged as heat regenerators, 5 a gas port operatively associated with each heat regenerator, and means associated with said gas ports adapted to establish a gas flow In testimony whereof I have hereunto set my hand.

ROLAND EDGAR SLADE. 

